Mulholland admitted on HDYSAPLM that when she first started out she had to sell her car after moving to London, to be able to afford to continue in her chosen career, so determined was she to succeed in London's West End. On achieving success Mulholland said in an interview, "If anyone had said a year ago that I'd be in one West End show, never mind two, I'd have never believed it," she said. "This all feels like a dream."[8][9][10]

On appearing in HDYSAPLM? Mulholland said, "It was very, very tough. My goal from the beginning had been to make it to the final and then let the public decide. So when I got voted out, I was absolutely devastated. I was so close and knocked at the final hurdle! It was a big shock to the system."[11] Andrew Lloyd Webber has since admitted that he made a mistake in sending her home too early from the BBC show, and is now immensely proud of the singer and her performances at the London Palladium as Maria; Lloyd Webber announced her recruitment saying her audition was "sensational."[12]

Shortly after HDYSAPLM finished in December 2006 Mulholland was signed by agents Curtis Brown and promptly took on the part of Roxie Hart, a lead character in the West End musical Chicago.[13] She received positive reviews in the Daily Mail,[14] Broadway.com and The Irish World.[15][16]

Mulholland left the cast of Chicago at the end of March 2007. That December, she was invited back to attend the 10 Year Charity Gala performance and Black Tie Reception to celebrate the production's tenth anniversary. Mulholland performed "Funny Honey" in duet with Denise van Outen.[17]

Although she did not win HDYSAPLM, Mulholland was asked by Andrew Lloyd Webber to take over the role of Maria in The Sound of Music as an 'alternate' on Monday evenings and Wednesday matinees from 16 April 2007, after the winner Connie Fisher had to scale down from eight to six performances a week following medical advice.[18] In the role of Maria, Mulholland has received strong reviews:[19] Megan Reynolds of The Guardian wrote that her performance was "honest, genuine, heartfelt and passionate, and her songs were pitch-perfect."[20] On 26 February 2008, Summer Strallen took over the role of Maria from Fisher. Mulholland continued to perform as the alternate until 20 August 2008.[21]

On Friday 24 August 2007 Mulholland performed at the BBC Radio 2 Gala for Andrew Lloyd Webber.[22] Mulholland sang "All The Love I Have" from The Beautiful Game. On 29 November 2007 Mulholland sang jazz and swing numbers at the 100 Club in London fronting the Sorrentino Band.[23] On Christmas Eve 2007, the BBC broadcast a show called When Joseph met Maria! in which she performed with Lee Mead and Connie Fisher and some of the other Maria and Joseph finalists in a BBC special.

Mulholland has represented Andrew Lloyd Webber's production The Sound of Music twice at the free event West End Live held in 2007 and 2008.[26] Between 3 and 5 July 2008, Mulholland starred in her own sold out show, Sway with Aoife, at the Town Hall Theatre, Galway. An album recorded during these shows was released on her website.[27] On 18 September 2008 Mulholland starred with the RTÉ Orchestra and Jessie Buckley in Dublin at the Concert Hall, in a Radio Broadcast highlighting songs from the career of Lloyd Webber, who joined her on stage.[28]

At the end of 2008, after leaving The Sound of Music, Mulholland presented a morning report on the Von Trapp family home for BBC Breakfast News. She also worked with the RTÉ children's television programme, Jam the Musical, as a mentor for a group of children rehearsing in a competition for a musical theatre performance.[citation needed]

She is comes from Salthill, a seaside resort in Galway, Ireland. Her grandparents owned a pub and her grandfather was often the main entertainer; Mulholland has said, "When her family get together there's always a sing-song. I come from a very musical family - every year we would meet on Christmas night and all the kids were encouraged to get up and perform. I think it was then that I realised I loved singing."[30] The first musical Mulholland appeared in was an amateur production of The Sound of Music, where she played Brigitta. Shortly before starting her course at the Central School of Speech and Drama, she moved to London and successfully auditioned for a part as a traditional Irish dancer, in the professional dance show, Dance of Desire, in which she spent four months. In 2003, she became the 30th annual 'Galway Rose', and represented Galway at The Rose of Tralee contest.[31]

On 6 September 2009 Mulholland married Jason Molins in Marbella, Spain, with her family and friends in attendance.[citation needed] She recently announced on her Facebook page that she is expecting her first child.

Mulholland has said her favourite character is Eliza Doolittle from My Fair Lady. "I love her transformation from a rough and ready girl to a sophisticated lady".[30] And she credits influences such as Julie Andrews, Judy Garland, and Dionne Warwick. She recalled the best piece of advice she received was: "Believe in yourself. There are plenty of people in life waiting to knock you down but if you have confidence in your talent, in your own ability, nobody can take that away from you and you will succeed. Never give up. Learn from your mistakes and move on."[32]